CHINESE JOURNAL OF CATALYSIS
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2025
·
IF 17.7
Mengyang Xu,Bingqing Chang,Jinze Li,Huiqin Wang,Pengwei Huo
The assembly of different Metal organic framework (MOFs) into hybrid heterostructures has proven to be a promising strategy that can effectively break through the limited regulatory capacity of single metal sites. Here, an S-scheme heterostructure (Fe 3 Ni-MOF) based on homologous ligands (1,4-phthalic acid) of ultra-thin Ni-MOF and Fe-MOF nanoparticles with directional electron transport channels, was developed and used it for photoreduction of CO 2 . Under the S-scheme electric field mechanism, the photogenerated carrier can achieve efficient directional separation through Fe–O–Ni atomic bond, which significantly reduces the energy barrier of the rate-determining step. Results show that the performance of Fe 3 Ni-MOF (63.5 μmol g –1 ) was 20 and 3.2 times higher than that of Ni-MOF and Fe-MOF, respectively, and exhibits excellent CO selectivity (96.4%) and stability. Transmission electron microscopy and atomic force microscopy revealed the two-molecular-layers structure of Ni-MOF and the micro-assembly structure of Fe 3 Ni-MOF, which can shorten the electron transport distance and increase the molecular mass transfer rate. X-ray photoelectron spectroscopy, electron spin resonance and electron density difference calculations reveal that interfacial electric fields and atomic bonds work together to promote directional carrier separation, resulting in the accumulation of holes on Ni-MOF and electrons on Fe-MOF. The Gibbs free energy calculation and in-situ Fourier transformed infrared spectroscopy validate that the micro-assembled S-scheme heterostructures with directional electron transport channels can significantly reduce the activation energy barrier of the reaction. This study not only proves the feasibility of constructing MOFs S-scheme heterostructures using homologous ligands, but also provides a new way to overcome the limitations of monometallic MOFs. This strategy is expected to open up a new avenue to design efficient photocatalysts.
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高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Yifan Li,Jiaxing Li,Lin Chen,Yunpeng Long,Xing Yuan,Junhua Li,Yue Peng
The low selectivity for N2 in the oxidation of NH3 over commercial Pt/Al2O3 catalysts is primarily due to the overoxidation of NH3 facilitated by Pt sites, leading to the formation of unwanted byproducts such as N2O and NO. In this study, we present a novel strategy to enhance N2 selectivity while maintaining NH3 conversion by constructing Pt–O–Cu dual sites. These dual sites exhibit synergistic acid-redox characteristics through surface electron transfer mediated by bridged lattice oxygen. Additionally, the ability of surface-adsorbed oxygen to exchange with lattice oxygen is significantly improved. The electron-deficient Cu sites enhance NH3 adsorption by providing empty 3d orbitals, while the electron-rich Pt sites promote NH3 dehydrogenation. Subsequently, the formation of –NH or –N intermediates at the Pt sites can react with adsorbed NH3 on the Cu sites to produce N2, predominantly following the integrated selective catalytic reduction mechanism. The optimized dual-site catalyst achieves over 95% NH3 conversion and N2 selectivity at 180 °C.
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高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Jianwei Xin,Irfan Muhammad,Zihui Meng,Yuqi Zhang
O-Phthalaldehyde (OPA) is a novel chemical disinfectant that has seen widespread use in healthcare environments. To ensure the efficacy of OPA-based disinfection in clinical practice, precise and reliable determination of its operational concentration is essential. Current methods, such as indicator strips, offer only semi-quantitative results, with their accuracy being influenced by multiple factors. Thus, there is an urgent need for the development of novel, efficient, and straightforward quantitative detection methods for OPA. DVD-R discs can be regarded as one-dimensional photonic crystals, which inspired the design of one-dimensional photonic crystal hydrogel (1DPCH) using DVD-R discs as templates. A sensor responsive to OPA was constructed by functionalizing the 1DPCH with ethylenediamine, thereby introducing amino groups into the hydrogel. These amino groups interact with OPA, and as the OPA concentration increases, the hydrogel undergoes enhanced crosslinking, leading to volume shrinkage. This shrinkage results in a reduction in the groove spacing of the embedded photonic crystal, which in increase the first-order diffraction spacing. By measuring the variation of the first-order diffraction spacing, the change in groove spacing can be quantified through a mathematical relationship. The experimental results exhibited a strong linear correlation with the change in groove spacing over the concentration logarithm range of 10 1 –10 6 nmol/L. the limit of detection was 1.26 nmol/L. additionally, the sensor exhibited high recovery rates (96.09–103.35 %) and low relative standard deviation (1.68–3.95 %) when detecting OPA in diluted disinfectant solutions. These findings suggest that the developed 1DPCH sensor is highly effective for the detection of OPA in clinical applications
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高影响因子
Advanced Science
·
2025
·
IF 14.1
Lili Liu,Chen Wang,Luxin Zhao,Yayun Xiao,Weiwei Fang,Lanling Zhao,Faxing Wang,Yuping Wu
The practical development of Li-O 2 batteries (LOBs) urgently needs to explore robust cathode catalysts to boost the sluggish Li 2 O 2 reaction kinetics and parasitic reactions despite their theoretically high specific energy. Profound understanding of the cathode properties and the battery performance is rather critical in developing rational-designed electrocatalysts. In this study, a Co-N x /Co (111) decorated N-doped hierarchical carbon framework (Co-N x /Co@NHCF) is proposed as an efficient cathode in LOBs. Spectroscopic analysis coupled with experimental results suggests that the Co-N x /Co (111) catalytic center can significantly reduce the battery overpotential, and meanwhile, the hierarchical carbon framework ensures rapid mass transportation and provides sufficient space to accommodate Li 2 O 2 deposition. Density functional theory calculations reveal that the incorporated Co (111) facet can effectively regulate the electronic distribution of N-carbon, optimize the adsorption of desirable intermediates, and eventually facilitate oxygen reduction reaction/oxygen evolution reaction kinetics. As expected, the Co-N x /Co@NHCF catalyzed LOBs deliver a high discharge/charge capacity of 6.15/ 6.22 mAh cm −2 with a columbic efficiency of 98.9%, along with a high rate cycling of 700 h at 0.3 mA cm −2 . This work provides valuable instruction for the rational design of efficient catalysts for high-performance LOBs via optimization of the crystal structure and the adsorption of intermediates.
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PubMed
高影响因子
ACS Nano
·
2025
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IF 16
Jimin Qiu,Yuchen Ji,Wenfang Li,Yuhang Li,Wenguang Zhao,Yunxing Zuo,Weiyuan Huang,Chen Zhu,Mingjian Zhang,Guorui Zheng,Luyi Yang,Feng Pan,Zu-Wei Yin
Lithium cobalt oxide (LiCoO2) cathodes suffer serious structure instability when charged to high voltage (>4.5 V), including H1-3 phase transition, cobalt dissolution, and interfacial side reactions, which are closely related to the instability of surface lattice oxygen. Herein, an interfacial B–O complexing strategy was proposed to stabilize the surface lattice oxygen of LiCoO2 at 4.6 V, through the preferential coordination between derived products of the tris(pentafluorophenyl)borane electrolyte additive and LiCoO2. Combining a series of in situ and ex situ characterization methods with temporal and spatial resolution, it was revealed that the emergence of peroxy-like species (O22–) at high potentials is one of the origins of the instability of LiCoO2, which can be well inhibited thanks to interfacial B–O complexing. Thus, oxygen loss and interfacial side reactions can be drastically retarded, which consequently provides a more stable chemical environment for Co element, avoiding the dissolution and valence reduction of Co. Owing to the well-anchored Co and O elements, undesirable phase transition and local coordination structure change are suppressed, hence improving the capacity retention and rate performance of LiCoO2 at 4.6 V. This study provides an interfacial complexing strategy to stabilize the high-voltage LiCoO2 cathode.
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PubMed
高影响因子
Journal of Materials Chemistry C
·
2016
·Vol. 4
·期 40
·9489-9498
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IF 5.066
Bo-Mei Liu,Zi-Jun Yong,Yang Zhou,Dan-Dan Zhou,Li-Rong Zheng,Li-Na Li,Hui-Mei Yu,Hong-Tao Sun
Bismuth-doped luminescent materials have gained significant attention in recent years owing to their huge potential for applications in telecommunications, biomedicine, and displays. However, controlled synthesis of these materials, in particular for those luminescing in the near-infrared (NIR) region, remains a challenging subject of continuous research efforts. Herein, we show that low-temperature topotactic reduction using Al metal powder as an oxygen getter can be adopted as a powerful technique for the conversion of bismuth-doped red-emitting systems into their NIR-emitting cousins. Thorough experimental characterization indicates that the framework oxygen of the hosts can be topotactically extracted, thus producing unique metal–oxygen–metal crystalline networks in reduced phases while preserving the crystalline structure of the precursor. For the first time, based on detailed analyses of X-ray absorption data, we identified that a minority of Bi atoms occupy Ba2+ sites, and most of the Bi atoms occupy the P5+ and/or B3+ sites in the as-synthesized Bi-doped BaBPO5. Subsequent topotactic treatment preferentially changes the local environment of Bi at the P5+/B3+ sites, which results in the occurrence of NIR emission owing to the birth of NIR-luminescent, defective Bi–O polyhedra in which Bi bears lower oxidation states with respect to that in the precursor. The site-specific topotactic reduction reaction reported here helps us create peculiar NIR-luminescent Bi–O units, and simultaneously does not seriously affect the red photoluminescence of Bi2+ situated at the Ba2+ sites. Given that the long-lived, ultrawide NIR emission covers the second biological window, the phosphors developed here hold great promise for in vivo luminescence and lifetime bioimaging. We anticipate that this low-temperature topotactic reduction strategy can be applied to the development of more novel Bi-doped luminescent materials in various forms that can find a broad range of functional applications.
研究领域:
材料科学
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光学
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生物医学工程
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2020
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IF 5.162
Yueping Jiang,Yanhong Feng,Bo Lei,Huiting Zhong
A compounded medium of supercritical CO 2 , ethanol, and water (SEW) was used to extract lignin from eucalyptus fiber and the mechanism of the extraction was studied. Compared with the extraction method based on high-temperature ethanol (HTE), the lignin yield of the SEW method was 49.7% higher with higher average molecular weight. Physical and chemical synergies occurred during the extraction process. SEW compound medium penetrated eucalyptus fiber cell walls because of strong permeability, while the fast discharge of the compounded medium facilitated efficient lignin dissociation and removal. Carbonic acid formed from CO 2 and water under high temperature and pressure can provide an acidic environment to effectively degrade hemicellulose . Formaldehyde formed from CO 2 and ethanol in the process also prevented condensation of the extracted lignin fragments. The obtained lignin had high content of β-O-4 linkages and syringyl units.
研究领域:
林产化学与工业
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生物质化学工程
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DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2019
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IF 3.774
Yun-Peng Zhao,Fa-Peng Wu,Qing-Lu Song,Xing Fan,Li-Jun Jin,Rui-Yu Wang,Jing-Pei Cao,Xian-Yong Wei
In this work, a bimetallic catalyst of Pd and Ni supported on HZSM-5 was designed and evaluated in the hydrodeoxygenation of model compounds representing various C–O bonds in lignin. The effects of temperature, holding time, and initial H 2 pressure on the catalytic performance of the Pd–Ni/HZSM-5 catalyst were investigated. The results indicated that the Pd–Ni/HZSM-5 catalyst exhibited superior catalytic activity towards the conversion of the model compounds to alkanes compared to its monometallic counterparts. Direct cleavage of the C–O bond in DPE was achieved under low H 2 pressure, mainly producing benzene and minor amounts of phenol and cyclohexane, while at high H 2 pressure, the reaction pathway was altered towards hydrogenation of the benzene ring , followed by then cleavage of the C–O bond to afford only cyclohexane. Moreover, the Pd–Ni/HZSM-5 catalyst showed high activities when applying other substrates including anisole, veratrole, guaiacol, benzyloxybenzene, phenethyl phenyl ether, and dibenzyl ether.
研究领域:
催化化学
·
能源化学
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高影响因子
JOURNAL OF CATALYSIS
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2020
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IF 7.888
Jie Zhang,Chuang Li,Weixiang Guan,Xiaozhen Chen,Xiao Chen,Chi-Wing Tsang,Changhai Liang
Co(Ni)/MoO 3 catalysts were prepared, characterized and evaluated for the hydrogenolysis of bio-derived dibenzofuran (DBF), aiming at the understanding of the promoting effect of Co/Ni on MoO 3 for high-yield production of aromatic products. All Co(Ni)/MoO 3 catalysts selectively cleaved C-O bond, thus effectively transformed DBF to biphenyl (BP) at relatively moderate conditions. The experimental results from varying Mo species by adjusting the reduction temperature of MoO 3 together with XPS and in-situ XRD characteristic were evident that Mo 5+ species was responsible as the major active specie for the reaction. Promotional effect between Co(Ni) and Mo in Co(Ni)/MoO 3 catalysts was observed, resulted from the presence of acidic Co(Ni)MoO 4 species and a large number of Mo 5+ species both of which were created local to the Co(Ni)-O-Mo interface, as can be characterized by in-situ XRD, XPS, H 2 -TPR, NH 3 -TPD, in-situ FT-IR, Raman and TEM. The trend of the initial reaction rate follows: MoO 3 (0.18 μmol∙g cat −1 ∙s −1 ) < Ni/MoO 3 (0.26 μmol∙g cat −1 ∙s −1 ) < Co/MoO 3 (0.29 μmol∙g cat −1 ∙s −1 ), corresponding to the decreasing activation barrier. And the best catalytic activity was observed for the 100% yield of BP over Co/MoO 3 . A possible mechanism, including Co(Ni) facilitated reduction of Mo 6+ to Mo 5+ and Co(Ni) enhanced formation of acidic sites, is proposed to be responsible for the high activity in Co(Ni)/MoO 3 catalysts.
研究领域:
催化化学
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可再生能源
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材料科学
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Jiacheng Xu,Tiantian Zhang,Yan Sun,Shiyu Fang,Zuliang Wu,Jiali Zhu,Lianxin Dai,Weihua Liu,Buhe Zhang,Junwei Zhang,Shuiliang Yao,Erhao Gao,Jing Li
MnO 2 is a promising catalyst due to its abundant metal valence and good redox ability. Different crystal phases of MnO 2 have different oxygen species, but the relationship between their catalytic activity and crystal structures is unclear. In this study, four MnO 2 catalysts with crystal structures ( α -, β -, γ -, and δ -MnO 2 ) were selected to unveil the roles of terminal-type (Mn O), superoxide-type Mn(-O-) 2 Mn, and bridge-type (Mn-O-Mn) oxygen species in CO oxidation . γ -MnO 2 has the best CO oxidation performance. Density functional theory calculation results show that Mn O on γ- MnO 2 can adsorb CO easier than other two types of oxygen species. Operando TPR-DRIFTS-MS results show that Mn O on the surface of γ- MnO 2 can react with CO to form terminal-type oxygen vacancies (M 2+ =□ 2– ) at low temperatures. Meanwhiles, Mn(-□-)(-O-)Mn and Mn-□-Mn can dissociate O 2 to form Mn O under certain conditions to promote CO oxidation. MnO 2 catalysts with more Mn O oxygen species are of great significance for CO oxidation at a low temperature.
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高影响因子
Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Qianyu Chu,Guangmin Ren,Jingdan Zhao,Xiangchao Meng,Jie Meng,Zizhen Li
The photocatalytic nitrogen reduction reaction (NRR) is a sustainable green alternative to the Haber–Bosch process for ammonia production. However, due to the inert properties of dinitrogen, the photocatalytic activity in N2 reduction is still pretty low. Based on density functional theory calculations, this study finds that the formation energy of oxygen vacancies around the V site in InVO4 was significantly lower than that around the In site. This indicated that the V–O bond was thermodynamically less stable and tends to break preferentially. Therefore, selective cleavage of the V–O bond was achieved by subjecting InVO4 to transient high-temperature treatment via rapid Joule heating technology. This resulted in the directed construction of an InVO4-JH catalyst enriched with oxygen vacancies and exposing coordination-unsaturated V sites. The resulting InVO4-JH catalyst delivered a photocatalytic ammonia production rate of up to 35.28 μmol g−1 h−1 under ambient conditions without any sacrificial agent, while exhibiting excellent stability and reaction selectivity. Mechanistic studies and structural characterization confirmed that the formation of oxygen vacancies via V–O bond cleavage releases electrons, which reduce adjacent V5+ to V4+. This created localized electron-rich regions at exposed V sites. Theoretical calculations further confirmed that these exposed V sites act as the active centers of the reaction, not only significantly enhancing nitrogen adsorption but also substantially lowering the energy barrier of the hydrogenation step through alternative reaction pathways. This work provides a novel strategy for the rational design of highly efficient defect-engineered catalysts via targeted bond cleavage.
研究领域:
材料化学
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光催化
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无机化学
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能源化学
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环境催化
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纳米材料
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表面科学
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DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Shanshan Shao,Tianrui Sun,Xiaohua Li,Yifan Wang,Laixin Ma,Zhufeng Liu,Shiliang Wu
Due to the high molecular weight, high viscosity and strong instability of heavy bio-oil from rape straw, it is necessary to explore new high-value utilization methods. Heavy bio-oil based carbon material (HBC) was prepared via carbonization and activation assisted by pyrolysis gas, and the basic Mg-Zr-O catalysts using HBC as the carrier (Mg-Zr-O/HBC) was synthesized for the aldol condensation of cyclopentanone to produce aviation fuel precursor. The effect of activation condition on the physicochemical properties of HBC and Mg-Zr-O/HBC were evaluated, the evolution of gas component before and after activation was explored, and the catalytic performance of Mg-Zr-O/HBC in the aldol condensation of cyclopentanone for the synthesis of aviation fuel was tested. Instead of traditional KOH activation, pyrolysis gas activation was beneficial for the reduced pollution and increased calorific value of the gas, making it an environmentally friendly method. The results showed that the activation of biochar (BOC) was improved with lower pyrolysis gas flow , higher activation temperature and longer activation time. The pore structure of carbon material was significantly improved, and the specific surface area was boosted from 15.25 m 2 /g 3 to 627.61 m 2 /g 3 . Mg-Zr-O was evenly distributed on HBC, and a large number of weak and medium basic sites were found in Mg-Zr-O/HBC, which was quite favorable for the aldol condensation. In the aldol condensation of cyclopentanone, Mg-Zr-O/HBC presented the excellent production of the targeted C10+C15 condensates of 84.95 %, which was comparable to that prepared with KOH as activator. After 8 repeated runs, the yield of the targeted condensates remained at 73.33 %. In general, it provided an environmentally friendly strategy for the preparation of HBC and the high-value utilization of pyrolysis gas assisted by pyrolysis gas for the activation of BOC.
研究领域:
能源科学
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催化化学
·
环境工程
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高影响因子
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